We investigated the effect of deposition temperature on the properties of the silicon oxide films produced by alternating exposures to bis(diethylamino)silane (BDEAS) and ozone (O₃). The surface reactions during the deposition were studied using in situ characterization techniques and density functional theory (DFT) calculations. The atomic layer deposition (ALD) temperature window was between 250 and 350 °C with a nearly constant growth rate of ∼ 0.10 nm/cycle and the step coverage higher than 94%. The saturation doses of BDEAS and O₃/O₂ were 5 × 10⁶ L and 5 × 10⁷ L. Among the films deposited in genuine ALD mode, the film deposited at 350 °C exhibited the lowest leakage current of 2.4 × 10^-8 A/cm² at −2 MV/cm and the lowest oxide trapped charge density of 6.5 × 10¹¹/cm². The in situ quartz crystal microbalance analysis showed that approximately 0.5 diethylamine ligand per BDEAS molecule was expected to remain on the surface after the BDEAS feeding. The in situ Fourier-transform infrared difference spectrum confirmed the presence of the ligand on the surface. DFT simulations showed that all NEt₂ ligands are released on vicinal and geminal hydroxyl groups to form –SiH₂*. However, only one NEt₂ ligand can be removed on isolated hydroxyls because no other hydroxyls are nearby, resulting in –SiH₂(NEt₂)*.

我们研究了沉积温度对交替暴露于双（二乙氨基）硅烷 (BDEAS) 和臭氧 (O ₃ ) 所产生的氧化硅薄膜性能的影响。使用原位表征技术和密度泛函理论 (DFT) 计算来研究沉积过程中的表面反应。原子层沉积 (ALD) 温度窗口在 250 到 350 °C 之间，生长速率几乎恒定，约为 0.10 nm/周期，阶梯覆盖率高于 94%。BDEAS和O ₃ /O ₂的饱和剂量分别为5×10 ⁶ L和5×10 ⁷L. 在真正的 ALD 模式沉积的薄膜中，在 350 °C 沉积的薄膜在 -2 MV/cm 时表现出最低的漏电流 2.4 × 10 ^-8 A/cm ²和最低的氧化物俘获电荷密度 6.5 × 10 ¹¹ /厘米²。该原位石英晶体微量天平分析表明，每分子BDEAS大约0.5二乙胺配体预期BDEAS馈送之后保持在表面上。该原位傅立叶变换红外差异光谱证实了表面上的配体的存在。DFT 模拟表明，所有 NEt ₂配体都在邻位和孪生羟基上释放，形成 –SiH ₂ *。然而，只有一个 NEt₂配体可以在孤立的羟基上去除，因为附近没有其他羟基，导致 –SiH ₂ (NEt ₂ )*。